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Bio-inspired construction of electrocatalyst decorated hierarchical porous carbon nanoreactors with enhanced mass transfer ability towards rapid polysulfide redox reactions

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Nano Research 2021年第11期14卷 3942-3951页

作者： Shijie Zhang Yongshang Zhang Guosheng Shao Peng Zhang School of Materials Science and Engineering Zhengzhou UniversityZhengzhou450001China State Centre for International Cooperation on Designer Low-Carbon&Environmental Materials(CDLCEM) Zhengzhou University100 Kexue AvenueZhengzhou450001China Zhengzhou Materials Genome Institute Building 2ZhongyuanzhiguXingyang450100China

Li-S batteries are considered as a highly promising candidate for the next-generation energy storage system, attributing to their tremendous energy density. However, the two-dimensional island nucleation-growth process of lithium sulfide leads to a thick insulating film covering the electrode, inducing slow electrons transfer and mass-transfer of ions and liquid sulfur species in working Li-S cells. Here, we demonstrate a bio-inspired strategy of constructing ant-nest-like hierarchical porous ultrathin carbon nanosheet networks with the implants of metallic nanoparticles electrocatalysts (HPC-MEC) as efficient nanoreactors enabling rapid mass transfer, via a simple and green NaCl template. Such nanoreactors with a large active surface area could effectively anchor polysulfides for mitigating the shuttle effect, facilitating uniformly thin Li2S film, and promoting the mass transfer for fast sulfur species conversions. This helps contribute to a continuously high sulfur utilization in Li-S batteries with the HPC-MEC reactors. As a typical exhibition, cobalt embedded hierarchical porous carbon (HPC-Co) could realize to deliver a remarkably high specific capacity of 1,540.6 mAh·g−1, an excellent rate performance of 878.8 mAh·g−1 at 2 C, and high area capacity of 11.6 mAh·cm−2 at a high sulfur load of 10 mg·cm−2 and low electrolyte/sulfur ratio of 5 µL·mg−1.

关键词： sulfur species reactor hierarchical porous carbon network electrocatalyst high sulfur loading low electrolyte/sulfur ratio

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EDTA-assisted hydrothermal synthesis of flower-like CoSe_2 nanorods as an efficient electrocatalyst for the hydrogen evolution reaction

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Journal of Energy Chemistry 2019年第1期28卷 95-100页

作者： Yanghui Deng Cui Ye Guo Chen Baixiang Tao Hongqun Luo Nianbing Li Key Laboratory of Eco-environments in Three Gorges Reservoir Region (Ministry of Education) School of Chemistry and Chemical Engineering Southwest University

Hydrogen evolution reaction(HER) is a prospective method to generate pure hydrogen. The development of superior electrocatalysts based on earth-abundant materials, plays a critical role in the ***_2, one of the earth-abundant electrocatalysts, has been proved to be a promising catalyst for hydrogen generation. In our work, flower-like CoSe_2 nanorods with high quality are successfully synthesized through a facile ethylenediaminetetraacetic acid ligand(EDTA)-assisted hydrothermal process. The flower-like CoSe_2 nanorods show the brilliant electrochemical HER performance with 100 mA cm^(-2) at overpotential of 273 m V, a small Tafel slope of 35 mV dec^(-1) and strong durability in acid solution. The sparkly HER catalytic activity of CoSe_2 can be ascribed to its particular structure with large surface area and abundant active sites. Therefore, this work offers an outstanding candidate for improving hydrogen production capabilities by water electrolysis.

关键词： Flower structure CoSe2 electrocatalyst Hydrogen evolution

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Synthesis and application of transition metal phosphides as electrocatalyst for water splitting

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Science Bulletin 2017年第9期62卷 633-644页

作者： Jinzhan Su Jinglan Zhou Lu Wang Cong Liu Yubin Chen International Research Center for Renewable Energy (IRCRE) State Key Laboratory for Multiphase Flow in Power Engineering Xi'an Jiaotong University Xi'an 710049 China

With continuous research on photocatalytic water splitting, searching for efficient catalyst for hydrogen evolution reaction(HER) becomes popular topic in addition to main catalyst research. Transition metal phosphides are receiving intense attention due to its abundance in the Earth's crust and comparable catalytic properties to noble metals. In this review, the synthesis approaches, HER reaction mechanism,photocatalytic activity, approaches to improve the activity of transition metal phosphides were reviewed and discussed. It was showed that the transition metal phosphides have great potential to reduce the cost of photocatalyst and promising application on water splitting. The stability problem and participation of poisonous reactant and product in its synthesis reaction limit its application and developing in a certain extent, but with the continuous efforts on the development and improvement of the synthesis methods,transition metal phosphides will find wide application in water splitting.

关键词： Transition metal phosphide electrocatalyst HER Photocatalytic water splitting

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Lignin derived multi-doped(N, S, Cl) carbon materials as excellent electrocatalyst for oxygen reduction reaction in proton exchange membrane fuel cells

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Journal of Energy Chemistry 2020年第5期29卷 106-114页

作者： Yixing Shen Yuhang Li Guangxing Yang Qiao Zhang Hong Liang Feng Peng School of Chemistry and Chemical Engineering Guangzhou UniversityGuangzhou 510006GuangdongChina School of Chemistry and Chemical Engineering South China University of TechnologyGuangzhou 510640GuangdongChina

Nowadays,hierarchically macro-/meso-/microporous 3D carbon materials have been paid more attention due to their imaginative application potential in specific ***,we report a dualtemplate strategy using eutectic NaCl/ZnCl2 melt as airtight and swelling agent to obtain 3D mesoporous skeleton structured carbon from renewable *** prepared lignin-derived biocarbon material(LN-3-1)has a high specific surface area(1289 m^2 g^-1),a large pore volume(2.80 cm^3 g^-1),and a well-connected and stable ***-3-1 exhibits extremely high activity and stability in acidic medium for oxygen reduction reaction(ORR),superior to Pt/C catalyst and most non noble-metal catalysts reported in recent *** prepared carbon material was used as a cathode catalyst to assemble a H2-O2 single fuel cell,and its excellent catalytic performance has been confirmed with the maximum power density of 779 mW cm^-2,which is one of the highest power densities among non-metallic catalysts so *** functional theory(DFT)calculations indicate that the synergy of chlorine and nitrogen reconciles the intermediate adsorption energies,leading to an appropriate theoretical ORR onset *** develop a cost-effective and highly efficient method to prepare biocarbon catalyst for ORR in proton-exchange membrane fuel cells.

关键词： electrocatalyst Biocarbon Fuel cells Lignin-derived carbon Oxygen reduction reaction Chlorine doping

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Facile synthesis based on novel carbon-supported cyanogel of structurally ordered Pd3Fe/C as electrocatalyst for formic acid oxidation

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Nano Research 2018年第9期11卷 4686-4696页

作者： Zhenyuan Liu Gengtao Fu Jiahui Li Zhenqi Liu Lin Xu Dongmei Sun Yawen Tang Jiangsu Key Laboratory of New Power Batteries Jiangsu Collaborative Innovation Centre of Biomedical Functional Materials School of Chemistry and Materials Science Nanjing Normal University Nanjing 210023 China School of Chemical and BiomedicalEngineering Nanyang Technological University Singapore 637459 Singapore

A novel carbon-supported cyanogel （C@cyanogel）-derived strategy is used to synthesize an intermetallic Pd3Fe/C compound of the desired ordered Pd3Fe phase with a small particle size. The novelty of this work lies in using carbon- supported K2PdHCl4/K4Fe^Ⅱ（CN）6 cyanogel as a reaction precursor, generated through the substitution of two chloride ligands by the nitrogen ends of the cyanide ligands on the metal center. The inherent nature of cyanogels can effectively suppress the movement of Pd^0 and Fe^0 nuclei in the crystal, benefiting the formation of the intermetallic, which is otherwise challenging via traditional synthesis techniques. The ordered Pd3Fe/C catalyst exhibits excellent catalytic activity and good cycle stability for the formic acid oxidation （FAO） reaction relative to the properties of disordered Pd3Fe/C and commercial Pd/C catalysts, dernonstrating that the ordered Pd3Fe/C is a promising replacement for commercial Pd-based catalysts. The outstanding performance can be ascribed to the full isolation of active sites in the ordered Pd3Fe structure and the modified electronic structure of the active components. This work provides an effective and novel route to obtain Pd-based intermetallic compounds with potential applications in a wide range of electrocatalysis.

关键词： carbon@cyanogel Pd3Fe/C ordered intermetallic electrocatalyst formic acid oxidation

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Controlled synthesis of ultrasmall RuP_(2) particles on N,P-codoped carbon as superior pH-wide electrocatalyst for hydrogen evolution

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Rare Metals 2021年第5期40卷 1040-1047页

作者： Ying-Hua Wang Rui-Qing Li Hai-Bo Li Hong-Li Huang Zeng-Jing Guo Hong-Yan Chen Yao Zheng Kong-Gang Qu School of Chemistry and Chemical Engineering Shandong Provincial Key Laboratory/Collaborative Innovation Center of Chemical Energy Storage and Novel Cell TechnologyLiaocheng UniversityLiaocheng 252059China School of Chemical Engineering and Advanced Materials The University of AdelaideAdelaideSA 5005Australia

Electrocatalytic hydrogen evolution reaction(HER)is a highly potential strategy to massively produce green hydrogen ***,the employment of costly Pt-based electrocatalyst in the cathode of electrolyzer greatly hampers the development of hydrogen *** phosphide catalysts have recently drawn wide attention due to the Pt-like activity but relatively lower ***,a facile strategy was proposed for the controlled preparation of the ultrasmall RuP_(2) nanoparticles on N,P-codoped carbon from common precursors of Ru(Ⅱ)complex and phytic *** taking advantage of simple mixing and pyrolysis,the as-synthesized RuP_(2) nanoparticles were uniformly embedded onto the N,P-codoped carbon *** composite catalyst shows better activity than Pt/C for alkaline HER and comparable activity for acidic and neutral *** superior activity can be ascribed to the ultrasmall-size and efficient RuP_(2) together with good mass and charge transfer ability assured by N,P-codoped carbon *** advantages including low-cost and simple synthesis in this work present an encouraging substitute to replace commercial Pt/C for hydrogen-related practical applications.

关键词： RuP_(2) N P-codoped carbon Hydrogen evolution electrocatalyst

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Defect and Doping Co‑Engineered Non‑Metal Nanocarbon ORR electrocatalyst

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Nano-Micro Letters 2021年第4期13卷 178-207页

作者： Jian Zhang Jingjing Zhang Feng He Yijun Chen Jiawei Zhu Deli Wang Shichun Mu Hui Ying Yang Key Laboratory of Material Chemistry for Energy Conversion and Storage Ministry of EducationSchool of Chemistry and Chemical EngineeringHuazhong University of Science and TechnologyWuhan 430074People’s Republic of China Pillar of Engineering Product Development Singapore University of Technology and Design8 Somapah RoadSingapore 487372Singapore State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070People’s Republic of China Foshan Xianhu Laboratory of the Advanced Energy Science and Technology Guangdong Laboratory Xianhu Hydrogen ValleyFoshan 528200People’s Republic of China

Exploring low-cost and earth-abundant oxygen reduction reaction(ORR)electrocatalyst is essential for fuel cells and metal–air *** them,non-metal nanocarbon with multiple advantages of low cost,abundance,high conductivity,good durability,and competitive activity has attracted intense interest in recent *** enhanced ORR activities of the nanocarbons are normally thought to originate from heteroatom(e.g.,N,B,P,or S)doping or various induced ***,in practice,carbon-based materials usually contain both dopants and *** this regard,in terms of the co-engineering of heteroatom doping and defect inducing,we present an overview of recent advances in developing non-metal carbon-based electrocatalysts for the *** characteristics,ORR performance,and the related mechanism of these functionalized nanocarbons by heteroatom doping,defect inducing,and in particular their synergistic promotion effect are emphatically analyzed and ***,the current issues and perspectives in developing carbon-based electrocatalysts from both of heteroatom doping and defect engineering are *** review will be beneficial for the rational design and manufacturing of highly efficient carbon-based materials for electrocatalysis.

关键词： Defect Doping electrocatalyst Oxygen reduction reaction Non-metal nanocarbon

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Inverted-design for highly-active hydrogen evolution electrocatalyst of MoS_(2)@Ni_(3)S_(2)core-shell via unlocking the potential of Mo

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Particuology 2023年第6期77卷 56-61页

作者： Chao Song Yuhua Liu Chengxiang Huang Miao Liu Nailin Yue Zunhao Zhang Zizhun Wang Xu Zou Wei Zhang Weitao Zheng Key Laboratory of Automobile Materials MOE School of Materials Science&EngineeringJilin Provincial International Cooperation Key Laboratory of High-Efficiency Clean Energy MaterialsElectron Microscopy CenterInternational Center of Future ScienceJilin UniversityChangchun130012China

Through inverted-design rather than modifying the generally-assumed S active sites in popular MoS_(2),we unlock the potential of Mo sites and successfully prepared novel MoS_(2)@Ni_(3)S_(2)/NF core-shell nanospheres as a catalyst for the high-performance hydrogen evolution reaction(HER).TheΔGH at the Mo site is optimized via Ni_(3)S_(2)to achieve excellent HER *** low current densities,it has similar activity to the Pt/***,its performance is better than Pt/C at high ***,our catalyst shows a considerable stability at a variety of current densities for 50 h,promising to substitute noble metal catalysts in application of commercial alkaline electrocatalysts.

关键词： Inverted design Hydrogen evolution reaction electrocatalyst Electronicinteraction MoS_(2)@Ni_(3)S_(2)/NF

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In situ sulfur-doped graphene nanofiber network as efficient metal-free electrocatalyst for polysulfides redox reactions in lithium–sulfur batteries

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Journal of Energy Chemistry 2020年第8期29卷 281-290,I0010页

作者： Shijie Zhang Peng Zhang Ruohan Hou Bin Li Yongshang Zhang Kangli Liu Xilai Zhang Guosheng Shao School of Materials Science and Engineering Zhengzhou UniversityZhengzhou 450001HenanChina State Centre for International Cooperation on Designer Low-Carbon&Environmental Materials(CDLCEM) Zhengzhou University100 Kexue AvenueZhengzhou 450001HenanChina Zhengzhou Materials Genome Institute Building 2ZhongyuanzhiguXingyang 450100HenanChina

The major challenge for realistic application of Li-S batteries lies in the great difficulty in breaking through the obstacles of the sluggish kinetics and polysulfides shuttle of the sulfur cathode at high sulfur loading for continuously high sulfur utilization during prolonged charge-discharge *** we demonstrate that large percentage of sulfur can be effectively incorporated within a three-dimensional(3D)nanofiber network of high quality graphene from chemical vapor deposition(CVD),through a simple ball-milling *** high quality graphene network provided continuous and durable channels to enable efficient transport of lithium ions and electrons,the in-situ sulfur doping from the alloying effect of ball milling facilitated desirable affinity with entire sulfur species to prevent sulfur loss and highly active sites to propel sulfur redox reactions over *** resulted in remarkable rate-performance and excellent cycling stability,together with large areal capacity at very high sulfur mass loading(Specific capacity over 666 mAh g-1after 300 cycles at 0.5 C,and areal capacity above 5.2 mAh cm-2at 0.2C at sulfur loading of 8.0 mg cm-2 and electrolyte/sulfur(E/S)ratio of 8μL mg-1;and high reversible areal capacities of 13.1 m Ah cm-2 at a sulfur load of 15 mg cm-2 and E/S of 5μL mg-1).

关键词： Lithium–sulfur–graphene batteries S-doped graphene electrocatalyst High sulfur loading Electrospinning

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High electrocatalytic hydrogen evolution activity on a coupled Ru and CoO hybrid electrocatalyst

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Journal of Energy Chemistry 2019年第10期28卷 143-147页

作者： Jia-Xin Guo Dong-Yang Yan Kang-Wen Qiu Chuan Mu Dian Jiao Jing Mao Hui Wang Tao Ling Key Laboratory for Advanced Ceramics and Machining Technology of Ministry of Education Tianjin Key Laboratory of Composite and Functional MaterialsSchool of Materials Science and EngineeringTianjin UniversityTianjin 300072China Key Laboratory of Aerospace Materials and Performance(Ministry of Education) School of Materials Science and EngineeringBeihang UniversityBeijing 100191China

Hydrogen evolution reaction (HER) is an essential step in converting renewable energy to clean hydrogen fuel. Exploring highly efficient, stable and cost-effective electrocatalysts is of crucial significance for sustainable HER. Here, we report the design of a coupled ruthenium/cobalt oxide (Ru/CoO) hybrid electrocatalyst for alkaline HER. In this hybrid metal/oxide system, the complicated alkaline HER pathways are overall facilitated;oxygen (O)-vacancy-abundant oxide enhances water splitting and Ru promotes successive hydrogen intermediates to generate hydrogen. The resulting Ru/CoO hybrid electrocatalyst exhibits significantly promoted catalytic activity compared with benchmark Ru catalyst, displaying an overpotential of 55 mV to generate a HER current density of 10 mA cm^-2, comparable with the state-of-the-art Pt/C catalyst and the most efficient alkaline HER electrocatalysts. Furthermore, the strong interaction of Ru nanoparticles with oxide support and the in-situ growth of oxide support on conductive substrate guarantee the long-term stability of as-fabricated Ru/CoO hybrid electrocatalyst. This newly designed hybrid catalyst with abundant metal/oxide interfaces may pave a new pathway for exploring efficient and stable HER electrocatalysts.

关键词： Ruthenium Oxides Hybrid electrocatalyst Hydrogen evolution reaction

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